Dynamic Behavior of Industrial Gas Phase Fluidized Bed Polyethylene Reactors under PI Control

A mathematical model describing the UNIPOL process for the production of polyethylene in the gas phase using a Ziegler‐Natta catalyst in a bubbling fluidized bed is used to analyze the major processes determining the behavior and performance of these industrially important units. The investigation shows that both static bifurcation (multiplicity of the steady states) as well as dynamic bifurcation (stable/unstable periodic attractors) behavior cover wide regions of the design and operating parameter domain. A conventional proportional‐integral (PI) control policy is suggested to stabilize the behavior of the system. The control philosophy covers both aspects of stabilizing unstable steady states as well as compensating for external disturbances. It is shown that for some controller configurations and set points the controlled process can go through a period doubling sequence leading to chaotic strange attractors. The industrial implications of the phenomena discovered for both the open loop (uncontrolled) as well the closed‐loop (controlled) systems are analyzed.     

Statistical Optimization for Production of Light Olefins in a Fluidized‐Bed Reactor

The methanol‐to‐olefins reaction (MTO) was studied in a small‐scale fluidized‐bed reactor over synthesized silicoaluminophosphate (SAPO‐34) catalysts. Mesoporous nanocrystalline SAPO‐34 molecular sieves were synthesized hydrothermally by ultrasonic and microwave‐assisted aging processes in the presence of hexadecyltrimethylammonium bromide (CTAB) and tetradecyldimethyl(3‐trimethoxysilylpropyl)ammonium chloride (TPOAC) as surfactant agents. The Box‐Behnken experimental design method was applied to determine the optimum operating parameters of this process conducted in the fluidized‐bed reactor. The optimum conditions in terms of reaction temperature, ratio of inlet gas velocity to minimum fluidizing velocity, and MeOH weight fraction were evaluated.     

Effect of Polymer Growth Rate and Diffusion Resistance on the Behavior of Industrial Polyethylene Fluidized Bed Reactor

The two‐phase model developed for the UNIPOL polyethylene process is improved by introducing polymer diffusion resistance, this means modelling of polyethylene fluidized bed reactors has been examined on two levels, at small scale of individual polymer particle, and macroscale of the whole reactor. The model utilizes the multigrain model that accounts for the reaction rate at catalyst surface to explore the static and dynamic bifurcation behavior of the fluidized bed catalytic reactor. Detailed bifurcation diagrams are developed and analyzed for the effect of polymer growth factor and Thiele modulus (the significance of the porous medium transport resistance is characterized by Thiele modulus) on reactor dense phase monomer concentration and reactor temperature as well as polyethylene production rate and reactor single pass conversion for the safe temperature region. The observations reveal that significant diffusion resistance to monomer transport exists, and this can mask the intrinsic rate constants of the catalyst. The investigation of polymer growth factor indicates that, the nascent stage of polymerization is highly gas phase diffusion influenced. Intraparticle temperature gradients would appear to be negligible under most normal operating conditions.     

A Novel Fluidized‐Bed Membrane Dual‐Type Reactor Concept for Methanol Synthesis

A novel fluidized‐bed membrane dual‐type methanol reactor (FBMDMR) concept is proposed in this paper. In this proposed reactor, the cold feed synthesis gas is fed to the tubes of the gas‐cooled reactor and flows in counter‐current mode with a reacting gas mixture in the shell side of the reactor, which is a novel membrane‐assisted fluidized bed. In this way, the synthesis gas is heated by heat of reaction which is produced in the reaction side. Hydrogen can penetrate from the feed synthesis gas side into the reaction side as a result of a hydrogen partial pressure difference between both sides. The outlet synthesis gas from this reactor is fed to tubes of the water‐cooled packed bed reactor and the chemical reaction is initiated by the catalyst. The partially converted gas leaving this reactor is directed into the shell of the gas‐cooled reactor and the reactions are completed in this fluidized‐bed side. This reactor configuration solves some drawbacks observed from the new conventional dual‐type methanol reactor, such as pressure drop, internal mass transfer limitations, radial gradient of concentration, and temperature in the gas‐cooled reactor. The two‐phase theory of fluidization is used to model and simulate the proposed reactor. An industrial dual‐type methanol reactor (IDMR) and a fluidized‐bed dual‐type methanol reactor (FBDMR) are used as a basis for comparison. This comparison shows enhancement in the yield of methanol production in the fluidized‐bed membrane dual‐type methanol reactor (FBMDMR).     

Experimental Study on Flow Behavior in a Gas‐Solid Fluidized Bed for the Methanol‐to‐Olefins Process

A cold model experimental system is established to investigate the flow behavior in a gas‐solid fluidized bed for the methanol‐to‐olefins process catalyzed by SAPO‐34. The system comprises a gas distributor in a F 300 × 5000 mm acrylic column, double fiber optic probe system and a series of cyclones. The experiments are carried out under conditions of atmospheric pressure and room temperature with different superficial velocities (0.3930–0.7860 m s^–1) and different initial bed heights (600–1200 mm). The effects of radial distance, axial distance, superficial gas velocity, and initial bed height on the solid concentration and particle velocity in the bed are discussed. The time‐averaged solid concentration and rising particle velocity profiles under different conditions are obtained. The results show that an increase in the value of r/R or initial bed height results in an increase in the solid concentration but a decrease in the rising particle velocity in the dense phase area, while improvement of the superficial gas velocity has a negative influence on the solid concentration but results in an increase in the rising particle velocity.     

Production of Electricity during Wastewater Treatment Using Fluidized‐Bed Microbial Fuel Cells

A membrane‐free fluidized‐bed microbial fuel cell (FB‐MFC) was applied to investigate the effects of fluidization parameters on its electrogenesis capacity. Active carbon particles were found to significantly decrease the start‐up time and increase the output voltage of the FB‐MFC. The fluidization behavior of the active carbon particles in the FB‐MFC reactor is one of the key parameters that influence the generation of electricity. With the FB‐MFC operating under optimal conditions, maximum power density with minimal internal resistance of the MFC could be obtained. The FB‐MFC could be operated in large‐scale wastewater treatment processes with high chemical oxygen demand removal efficiencies.     

Bubbling and Bed Expansion Behavior Under Vibration in a Gas‐Solid Fluidized Bed

The effect of vibration on the flow patterns and fluidization characteristics including the minimum fluidization velocity (u_mf), the void fraction (ϵ_mf) at u_mf and the bed expansion ratio were examined. The powders used were spherical glass beads and their diameters were 6, 20, 30, 60 and 100μm. For group A powders, the manner in which the vibration affects the bubble formation was examined from the bed expansion ratio and the index of n/4.65. The area of the homogeneous fluidization region was also observed. The homogeneous fluidization region was broadened at a certain vibration strength, where the value of n/4.65 was a minimum. The bubble formation was observed even for 20μm powder (group C), at large vibration strengths and at high gas velocities. Under such conditions, the bed expansion ratio increased suddenly due to bubble formation. The bubbles broke the irregular bed structure, including various properties of agglomerates. Although the channel breakage was dominant flow pattern for group C powders, the bubbles also played an important role in the improvement of the fluidization.     

Expansion Behavior of a Binary‐Solid Liquid Fluidized Bed with Large Particle Size Difference

The overall expansion of two dissimilar solid particle species with over a tenfold difference in their size and substantial density difference is investigated here for different compositions of the fluidized bed. Contrary to the widely held notion that the total bed height would be the sum of the heights of the two segregated mono‐component beds, the actual bed heights were, in fact, found to be lower. This volume contraction is found to strongly depend upon the mixing behavior prevailing in the binary‐solid fluidized bed. At the complete mixing of the two solid species, the bed‐contraction versus liquid velocity profile shows a global maximum. As a result, the overall bulk density profiles are similarly affected. Moreover, it is found here that correlations meant for predicting the porosity of the packing of binary particle mixtures can be satisfactorily extended to binary‐solid fluidized beds where solid species differ significantly in size.     

Experimental Investigations of Catalytic Partial Oxidation of Methane to Synthesis Gas in Various Types of Fluidized‐Bed Reactors

The partial oxidation of methane to synthesis gas over Ni/α‐Al₂O₃ catalysts (1 and 5 wt.‐% Ni loading, 71–160 and 250–355 μm particle diameter) was investigated in different types of fluidized‐bed reactors, i.e., the bubbling fluidized bed (FlB), the spout fluid bed (SFB) and the internally circulating fluidized bed (ICFB). A methane‐to‐oxygen ratio of 2:1 was used in all experiments and the temperature was varied between 700 and 800 °C. Gas velocities and catalyst masses were adjusted to assure a stable and controllable reactor operation. A nearly isothermal operation was established in all reactors. The thermodynamic equilibrium values were achieved in the FlB and SFB reactor whereas in the ICFB reactor slightly lower conversions and selectivities were obtained. Taking the direct scale‐up concept of the ICFB reactor into account, significant higher space‐time yields were obtained in this reactor than in the industrial‐scale bubbling fluidized‐bed reactor. No increase of the space‐time yield in comparison to the FlB was obtained in the SFB reactor.     

Volumetric Heat Transfer Coefficient in Fluidized‐Bed Dryers

In literature, there are several Nu=f(Re) equations to specify the heat transfer coefficient between solids and the drying gas, but these equations differ significantly because of the inaccuracy of determining the contact surface between the two phases. A pilot‐plant fluidized‐bed dryer is developed to study the heat and mass transfer phenomena during the drying process. A volumetric heat transfer coefficient is applied for modeling fluidized‐bed dryers. A modified Nusselt number is defined to compare the experimental results and those of the literature. The modified Nu'=f(Re) equation exhibits a proper correlation between the results of the experiments in the literature and those of our experiments.     

Manufacture of Granular Polysilicon from Trichlorosilane in a Fluidized‐Bed Reactor

Manufacturing of polysilicon by chemical vapor deposition from SiHCl₃ in a fluidized‐bed reactor was studied. The effects of reaction temperature, H₂/SiHCl₃ ratio, gas velocity, and seed particle loading were evaluated. The outlet gas composition was analyzed by gas chromatography. The physical features of the product particles were determined by scanning electron microscopy and laser particle size analyzer. Well‐grown product particles were obtained. The temperature and H₂/SiHCl₃ ratio significantly affected conversion, yield, and selectivity, which were less affected by gas velocity and seed particle loading at higher temperatures. The surface reaction kinetics determined the product yield only at lower temperatures, and thermodynamic equilibrium was approached at temperatures above 900 °C.     

Effects of Chaotic Temperature Fluctuations on the Heat Transfer Coefficient in Liquid‐Liquid‐Solid Fluidized Beds

The effect of chaotic temperature fluctuations on the immersed heater‐to‐bed heat transfer coefficient (h) are investigated in a liquid‐liquid‐solid fluidized bed (0.152 m ID × 2.5 m in height). The time series of temperature fluctuations are measured and analyzed by means of the multidimensional phase space portraits and Kolmogorov entropy (K), in order to characterize the chaotic behavior of heat transfer coefficient fluctuations in the bed. The overall heat transfer coefficient is inversely proportional to the Kolmogorov entropy of temperature fluctuations, as well as the fluctuation range of heat transfer coefficient (Δh_i). The Kolmogorov entropy and fluctuation range of the heat transfer coefficient (Δh_i) increase with increasing dispersed phase velocity, but decrease with increasing particle size. However, they attain their minima with variation of the continuous phase velocity as well as the bed porosity, at which point the flow regime of particles in the beds changes. The overall heat transfer coefficient is directly correlated with the Kolmogorov entropy, as well as the fluctuation range of heat transfer coefficient.     

Catalytic Oxidation of Methanol to Formaldehyde in a Continuous Fluidized‐Bed Reactor

Partial oxidation of methanol to formaldehyde by using a mixture of ferric and molybdenum oxides as the reaction catalyst at 280–330 °C has been studied in a continuous fluidized bed reactor. The reactor was a cylindrical tube of 20 mm in i.d. and 36 mm in o.d. placed vertically and connected to a truncated coneshaped cyclone separator. The catalyst was prepared by the precipitation method using aqueous solutions of ammonium heptamolybdate and ferric nitrate. The effect of certain parameters, such as temperature, superficial gas velocity and feed flow rates, on the extent of oxidation reaction has been investigated. The maximum size of the catalyst particles was 990 μm, therefore, neither external nor internal diffusion was expected to be effective in the process. The experimental data were correlated with three classes of hydrodynamic models presented for fluidized systems. The best correlation was obtained with compartment type models.     

Critical Bed Height for Solid Circulation in a Compartmented Gas‐Fluidized Bed

The influence of design and operating parameters on minimum upstream bed height required for steady solid circulation across a compartmented gas‐fluidized bed has been studied. The partition plate in the compartmented bed is fitted with two pairs of V‐valve and riser with orifices in them. Silica sand of three different sizes, viz., 490 μm, 325 μm and 250 μm, has been used and the range of the aeration rate tested covers 1–3U_mf through the bed, 5–60U_mf through the V‐valve and 0–60U_mf through the riser. A model incorporating pressure balance across the circulation loop has been developed to analyze the experimental findings. Studies show the existence of a unique critical bed height for a given set of fluidization velocities through the bed, V‐valve, riser and the size of the solids.     

Biological Nutrient Removal Using a Novel Laboratory‐Scale Twin Fluidized‐Bed Bioreactor

The capability of biological nutrient removal from wastewater of a novel laboratory‐scale twin fluidized‐bed bioreactor (TFBBR) was studied. The work showed approximately 96 % organic matter, 84 % nitrogen, and 12 % phosphorus removal efficiencies in the first three phases of the study at influent synthetic municipal wastewater (SMW) flow rates of 150, 190, and 240 L/d, with corresponding organic loading rates of 1.3, 1.7, and 2.3 kg COD m^–3 d^–1 and nitrogen loading rates of 0.14, 0.18 and 0.25 kg N m^–3 d^–1. The TFBBR effluent was characterized by <1.0 mg NH₄‐N/L, <4.3 mg NO₃‐N/L, <6 mg TN/L, <6 mg SBOD/L, and 6–10 mg VSS/L. For the three phases, biomass yields of 0.06, 0.066, and 0.071 g VSS/g COD were observed, respectively, which was a significant further reduction in yield compared to the liquid‐solid circulating fluidized‐bed bioreactor technology developed and patented by this research group, of 0.12–0.16 g VSS/g COD. The very low yield was due to a longer solid retention time of 72–108 d.     

The Segregation in the Binary‐Solid Liquid Fluidized Bed

A new mechanism is proposed to interpret the phenomena observed in the liquid fluidization of the binary particle mixture. Two main factors, the bulk density and voidage fluctuation, are considered to determine the position of the layer of particles in the bed. The new model successfully explains the layer inversion phenomenon and mixing‐segregation equilibrium, which is the result of the above two factors acting together. The model also proves that bulk density is a simple and reliable method to predict the inversion velocity by comparison with the experimental results reported in the literature.     

Bed Expansion – Extending Correlations for Fluidized Beds with Inserts to Open Fluidized Beds

Bed expansion occurs during the operation of gas‐fluidized beds and is influenced by particle properties, gas properties and distributor characteristics. It has a significant bearing on heat and mass transfer phenomena within the bed. A method of predicting bed expansion behavior from other fluidizing parameters would be a useful tool in the design process, dispensing with the need for small‐scale trials. This study builds on previous work on fluidized beds with vertical inserts to produce a correlation that links a modified particle terminal velocity, minimum fluidizing velocity and distributor characteristics with bed voidage in the relationship with P as the pitch between holes in the perforated distributor plate.     

Thermochemical Processing of Miscanthus through Fluidized‐Bed Fast Pyrolysis: A Parametric Study

Thermochemical processing of agriculture waste not only provides surrogates for combustion fuel but also reduces the environmental issues of waste. Miscanthus has been viewed as one of the largest agriculture wastes in Taiwan and a proper process for turning Miscanthus into a valuable product has become a significant subject. Here, fluidized‐bed fast pyrolysis was applied to convert Miscanthus into bio‐oil, bio‐char, and pyrolytic gases as the products. The product distributions were examined depending on various reaction parameters such as reaction temperature, carrier gas flow rate, feedstock feeding rate, and feedstock size. The chemical compositions of the bio‐oil, bio‐char, and product gases were analyzed and the properties of the bio‐oil were also tested via standard methods. So far, bio‐oil derived from Miscanthus is unfavorable for application in combustion engines without further upgrading processes.